# US 5,703,003 A · Durable regenerable sorbent pellets for removal of hydrogen sulfide from coal gas

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- Number: US 5,703,003 A
- Document ID: US5703003A
- Status: Granted
- Kind: A
- Application number: 08/562,538
- Filed: 1995-11-01
- Granted: 1997-12-30
- Earliest claimed: 1994-03-23
- Assignees: United States Department of Energy
- Inventors: Ranjani V. Siriwardane
- Web page: https://patentgrep.com/patent/US5703003A

## CPC

- B01J 20/28004: {Sorbent size or size distribution, e.g. particle size}
- B01D 53/02: by adsorption, e.g. preparative gas chromatography {(solid sorbent compositions B01J20/00, preparation of inorganic compounds or elements C01)}
- B01D 53/52: Hydrogen sulfide
- B01D 53/81: Solid phase processes
- B01J 20/06: comprising oxides or hydroxides of metals not provided for in group B01J20/04
- B01J 20/2803: {Sorbents comprising a binder, e.g. for forming aggregated, agglomerated or granulated products}
- B01J 20/28059: {being less than 100 m2/g}
- B01J 20/30: Processes for preparing, regenerating, or reactivating
- C10K 1/20: by treating with solids; Regenerating spent purifying masses {(separation by adsorption B01D53/02; separation by chemical reaction B01D53/34; refining of hydrocarbon oils with acids C10G17/02, C10G27/02, C10G29/12)}
- C10K 1/32: with selectively adsorptive solids, e.g. active carbon
- C10K 1/34: by catalytic conversion of impurities to more readily removable materials
- B01D 2257/304: Hydrogen sulfide
- Y02E 20/18: Integrated gasification combined cycle [IGCC], e.g. combined with carbon capture and storage [CCS]
- Y10S 502/517: Sulfur or sulfur compound removal
- B01J: CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
- B01D: SEPARATION (separating solids from solids by wet methods B03B, B03D; by pneumatic jigs or tables B03B; by other dry methods B07; magnetic or electrostatic separation of solid materials from solid materials or fluids, separation by high-voltage electric fields B03C; centrifuges, vortex apparatus B04; presses per se for squeezing-out liquid from liquid-containing material B30B9/02; treatment of water C02F, e.g. softening by ion-exchange C02F1/42; {arrangements of air intake cleaners in gas turbine plants F02C7/05} ; arrangements or mounting of filters in air-conditioning, air-humidification or ventilation F24F13/28)
- C10K: PURIFYING OR MODIFYING THE CHEMICAL COMPOSITION OF COMBUSTIBLE GASES CONTAINING CARBON MONOXIDE
- Y02E: REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
- Y10S: TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS

## Abstract

Pellets for removing hydrogen sulfide from a coal gasification stream at an elevated temperature are prepared in durable form usable over repeated cycles of absorption and regeneration. The pellets include a material reactive with hydrogen sulfide, in particular zinc oxide, a binder, and an inert material, in particular calcium sulfate (drierite), having a particle size substantially larger than other components of the pellets. A second inert material and a promoter may also be included. Preparation of the pellets may be carried out by dry, solid-state mixing of components, moistening the mixture, and agglomerating it into pellets, followed by drying and calcining. Pellet size is selected, depending on the type of reaction bed for which the pellets are intended. The use of inert material with a large particle size provides a stable pellet structure with increased porosity, enabling effective gas contact and prolonged mechanical durability.

## Claims

### Claim 1

Durable sorbent pellets chemically and physically stable for use in multi-cycle sulfidation and regeneration processes at temperatures over 260.degree. C. (500.degree. F.) consisting of a mixture of the following components:
a material reactive with hydrogen sulfide and selected from the group consisting of metal oxides, acetates, formates, carbonates ad nitrates of zinc, copper, iron, manganese, chromium, and mixtures thereof and having a particle size below 50 microns--30 to 65 weight percent;
a diluent selected from the group consisting of, calcium sulfate, calcium phosphate, magnesium sulfate, and zinc silicate, and having a particle size less than 50 microns--20 to 40 weight percent;
an inert material comprising particles having a particle size at least twice that of said material reactive with hydrogen sulfide selected from the group consisting of silica, silica gel, alumina, alumina gel, calcium sulfate (drierite), zinc silicate, and sand, wherein the particle size of said inert material is chosen to create additional voids between the components, thus increasing the porosity of the sorbent pellets --2 to 40 weight percent;
a binder unreactive with hydrogen sulfide, having a particle size less than said inert material, and selected from the group consisting of bentonite, kaolinite, and cement and mixtures thereof--2 to 45 weight percent;
a promoter selected from the group consisting of oxides and salts of copper, cobalt, manganese, nickel and mixtures thereof--an amount greater than zero and up to 10 weight percent;
said mixture having been moistened with water, formed into pellets, dried, and calcined at a temperature above 538.degree. C. (1,000.degree. F.), but low enough to avoid a chemical reaction of said material reactive with hydrogen sulfide with said diluent; and
said material reactive with hydrogen sulfide being unreactive with all other components of said mixture at said calcination temperature.

### Claim 2 (depends on 1)

Pellets as defined in claim 1 wherein said material reactive with hydrogen sulfide is zinc oxide.

### Claim 3 (depends on 1)

Pellets as defined in claim 1 wherein said inert material is calcium sulfate (drierite).

### Claim 4 (depends on 1)

Pellets as defined in claim 1 wherein said diluent is calcium sulfate.

### Claim 5 (depends on 1)

Pellets as defined in claim 1 wherein said inert material comprises at least 20 percent of particles at least 2 times larger than the particle size of said material reactive with hydrogen sulfide.

### Claim 6 (depends on 5)

Pellets as defined in claim 5 wherein said inert material comprises particles falling within a plurality of size fractions, one of which comprises particles at least twice the particle size of said material reactive with hydrogen sulfide.

### Claim 7 (depends on 1)

Pellets as defined in claim 1 comprising pellets having a size in the range of 2 mm to 5 mm and wherein the starting particle size of said inert material comprises particles over 50 microns in diameter.

### Claim 8 (depends on 7)

Pellets as defined in claim 7 wherein the particle size of said inert material is within the range of 75 to 700 microns.

### Claim 9 (depends on 1)

Pellets as defined in claim 1 comprising pellets having a size below 500 microns and wherein the size of the said inert material comprises less than 150 microns in diameter.

### Claim 10 (depends on 9)

Pellets as defined in claim 9 wherein the particle size of said inert material is from 5 to 100 microns.

### Claim 11

Durable sorbent pellets chemically and physically stable for use in multi-cycle sulfidation and regeneration processes at temperatures over 260.degree. C. (500.degree. F.) consisting of a mixture of the following components:
a material reactive with hydrogen sulfide and selected from the group consisting of metal oxides, acetates, formates, carbonates and nitrates of zinc, copper, iron, manganese, chromium, and mixtures thereof and having a particle size below 50 microns--30 to 65 weight percent;
an inert material comprising particles having a particle size at least twice that of said material reactive with hydrogen sulfide selected from the group consisting of silica, silica gel, alumina, alumina gel, calcium sulfate (drierite), zinc silicate, and sand, wherein the particle size of said inert material is chosen to create additional voids between the components, thus increasing the porosity of the sorbent pellets--2 to 40weight percent;
a binder unreactive with hydrogen sulfide, having a particle size less than said inert material, and selected from the group consisting of bentonite, kaolinite, and cement and mixtures thereof--2 to 60 weight percent;
said mixture having been moistened with water, formed into pellets, dried, and calcined at a temperature above 538.degree. C. (1,000.degree. F.); and
said material reactive with hydrogen sulfide being unreactive with all other components of said mixture at said calcination temperature.